New Energy Materials Laboratory, Sichuan Changhong Electronic (Group) Co.; Ltd., Chengdu, 610041, China.
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Nat Commun. 2023 Jun 16;14(1):3592. doi: 10.1038/s41467-023-38600-8.
Photocatalytic hydrogen evolution efficiency is limited due to unfavorable carrier dynamics and thermodynamic performance. Here, we propose to introduce electronegative molecules to build an electric double layer (EDL) to generate a polarization field instead of the traditional built-in electric field to improve carrier dynamics, and optimize the thermodynamics by regulating the chemical coordination of surface atoms. Based on theoretical simulation, we designed CuNi@EDL and applied it as the cocatalyst of semiconductor photocatalysts, finally achieved a hydrogen evolution rate of 249.6 mmol h g and remained stable after storing under environmental conditions for more than 300 days. The high H yield is mainly due to the perfect work function, Fermi level and Gibbs free energy of hydrogen adsorption, improved light absorption ability, enhanced electron transfer dynamics, decreased HER overpotential and effective carrier transfer channel arose by EDL. Here, our work opens up new perspectives for the design and optimization of photosystems.
由于载流子动力学和热力学性能不理想，光催化析氢效率受到限制。在这里，我们提出引入电负性分子构建电双层（EDL）以产生极化场来代替传统的内置电场，从而提高载流子动力学，并通过调节表面原子的化学配位来优化热力学。基于理论模拟，我们设计了 CuNi@EDL 并将其用作半导体光催化剂的助催化剂，最终实现了 249.6 mmol h g 的析氢速率，并且在环境条件下储存超过 300 天后仍保持稳定。高的 H 产率主要归因于 EDL 引起的完美功函数、费米能级和氢吸附吉布斯自由能、增强的光吸收能力、增强的电子转移动力学、降低的 HER 过电势和有效的载流子转移通道。在这里，我们的工作为光系统的设计和优化开辟了新的视角。
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